Light-Induced Halide Segregation in 2D and Quasi-2D Mixed-Halide Perovskites

Kunal Datta; Alessandro Caiazzo; Michael A. Hope; Junyu Li; Aditya Mishra; Manuel Cordova; Zehua Chen; Lyndon Emsley; Martijn M. Wienk; René A.J. Janssen

doi:10.1021/acsenergylett.3c00160

Light-Induced Halide Segregation in 2D and Quasi-2D Mixed-Halide Perovskites

Kunal Datta, Alessandro Caiazzo, Michael A. Hope, Junyu Li, Aditya Mishra, Manuel Cordova, Zehua Chen, Lyndon Emsley, Martijn M. Wienk, René A.J. Janssen (Corresponding author)

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Photoinduced halide segregation hinders widespread application of three-dimensional (3D) mixed-halide perovskites. Much less is known about this phenomenon in lower-dimensional systems. Here, we study photoinduced halide segregation in lower-dimensional mixed iodide-bromide perovskites (PEA₂MA_n-1Pb_n(Br_xI_1-x)_3n+1, with PEA⁺: phenethylammonium and MA⁺: methylammonium) through time-dependent photoluminescence (PL) spectroscopy. We show that layered two-dimensional (2D) structures render additional stability against the demixing of halide phases under illumination. We ascribe this behavior to reduced halide mobility due to the intrinsic heterogeneity of 2D mixed-halide perovskites, which we demonstrate via ²⁰⁷Pb solid-state NMR. However, the dimensionality of the 2D phase is critical in regulating photostability. By tracking the PL of multidimensional perovskite films under illumination, we find that while halide segregation is largely inhibited in 2D perovskites (n = 1), it is not suppressed in quasi-2D phases (n = 2), which display a behavior intermediate between 2D and 3D and a peculiar absence of halide redistribution in the dark that is only induced at higher temperature for the quasi-2D phase.

Originele taal-2	Engels
Pagina's (van-tot)	1662-1670
Aantal pagina's	9
Tijdschrift	ACS Energy Letters
Volume	8
Nummer van het tijdschrift	4
DOI's	https://doi.org/10.1021/acsenergylett.3c00160
Status	Gepubliceerd - 14 apr. 2023

Bibliografische nota

Funding Information:
The authors acknowledge funding of the research by The Netherlands Organization for Scientific Research (NWO) through the Joint Solar Programme III (Project 680.91.011) and the Spinoza prize, and by the Ministry of Education, Culture and Science (Gravity program 024.001.035). This work was supported by the Swiss National Science Foundation, grant number 200020_212046. M.A.H. acknowledges a H2020 MSCA fellowship (grant number 101024144).

Financiering

The authors acknowledge funding of the research by The Netherlands Organization for Scientific Research (NWO) through the Joint Solar Programme III (Project 680.91.011) and the Spinoza prize, and by the Ministry of Education, Culture and Science (Gravity program 024.001.035). This work was supported by the Swiss National Science Foundation, grant number 200020_212046. M.A.H. acknowledges a H2020 MSCA fellowship (grant number 101024144).

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title = "Light-Induced Halide Segregation in 2D and Quasi-2D Mixed-Halide Perovskites",

abstract = "Photoinduced halide segregation hinders widespread application of three-dimensional (3D) mixed-halide perovskites. Much less is known about this phenomenon in lower-dimensional systems. Here, we study photoinduced halide segregation in lower-dimensional mixed iodide-bromide perovskites (PEA2MAn-1Pbn(BrxI1-x)3n+1, with PEA+: phenethylammonium and MA+: methylammonium) through time-dependent photoluminescence (PL) spectroscopy. We show that layered two-dimensional (2D) structures render additional stability against the demixing of halide phases under illumination. We ascribe this behavior to reduced halide mobility due to the intrinsic heterogeneity of 2D mixed-halide perovskites, which we demonstrate via 207Pb solid-state NMR. However, the dimensionality of the 2D phase is critical in regulating photostability. By tracking the PL of multidimensional perovskite films under illumination, we find that while halide segregation is largely inhibited in 2D perovskites (n = 1), it is not suppressed in quasi-2D phases (n = 2), which display a behavior intermediate between 2D and 3D and a peculiar absence of halide redistribution in the dark that is only induced at higher temperature for the quasi-2D phase.",

author = "Kunal Datta and Alessandro Caiazzo and Hope, {Michael A.} and Junyu Li and Aditya Mishra and Manuel Cordova and Zehua Chen and Lyndon Emsley and Wienk, {Martijn M.} and Janssen, {Ren{\'e} A.J.}",

note = "Funding Information: The authors acknowledge funding of the research by The Netherlands Organization for Scientific Research (NWO) through the Joint Solar Programme III (Project 680.91.011) and the Spinoza prize, and by the Ministry of Education, Culture and Science (Gravity program 024.001.035). This work was supported by the Swiss National Science Foundation, grant number 200020_212046. M.A.H. acknowledges a H2020 MSCA fellowship (grant number 101024144). ",

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doi = "10.1021/acsenergylett.3c00160",

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AU - Datta, Kunal

AU - Caiazzo, Alessandro

AU - Hope, Michael A.

AU - Li, Junyu

AU - Mishra, Aditya

AU - Cordova, Manuel

AU - Chen, Zehua

AU - Emsley, Lyndon

AU - Wienk, Martijn M.

AU - Janssen, René A.J.

N1 - Funding Information: The authors acknowledge funding of the research by The Netherlands Organization for Scientific Research (NWO) through the Joint Solar Programme III (Project 680.91.011) and the Spinoza prize, and by the Ministry of Education, Culture and Science (Gravity program 024.001.035). This work was supported by the Swiss National Science Foundation, grant number 200020_212046. M.A.H. acknowledges a H2020 MSCA fellowship (grant number 101024144).

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N2 - Photoinduced halide segregation hinders widespread application of three-dimensional (3D) mixed-halide perovskites. Much less is known about this phenomenon in lower-dimensional systems. Here, we study photoinduced halide segregation in lower-dimensional mixed iodide-bromide perovskites (PEA2MAn-1Pbn(BrxI1-x)3n+1, with PEA+: phenethylammonium and MA+: methylammonium) through time-dependent photoluminescence (PL) spectroscopy. We show that layered two-dimensional (2D) structures render additional stability against the demixing of halide phases under illumination. We ascribe this behavior to reduced halide mobility due to the intrinsic heterogeneity of 2D mixed-halide perovskites, which we demonstrate via 207Pb solid-state NMR. However, the dimensionality of the 2D phase is critical in regulating photostability. By tracking the PL of multidimensional perovskite films under illumination, we find that while halide segregation is largely inhibited in 2D perovskites (n = 1), it is not suppressed in quasi-2D phases (n = 2), which display a behavior intermediate between 2D and 3D and a peculiar absence of halide redistribution in the dark that is only induced at higher temperature for the quasi-2D phase.

AB - Photoinduced halide segregation hinders widespread application of three-dimensional (3D) mixed-halide perovskites. Much less is known about this phenomenon in lower-dimensional systems. Here, we study photoinduced halide segregation in lower-dimensional mixed iodide-bromide perovskites (PEA2MAn-1Pbn(BrxI1-x)3n+1, with PEA+: phenethylammonium and MA+: methylammonium) through time-dependent photoluminescence (PL) spectroscopy. We show that layered two-dimensional (2D) structures render additional stability against the demixing of halide phases under illumination. We ascribe this behavior to reduced halide mobility due to the intrinsic heterogeneity of 2D mixed-halide perovskites, which we demonstrate via 207Pb solid-state NMR. However, the dimensionality of the 2D phase is critical in regulating photostability. By tracking the PL of multidimensional perovskite films under illumination, we find that while halide segregation is largely inhibited in 2D perovskites (n = 1), it is not suppressed in quasi-2D phases (n = 2), which display a behavior intermediate between 2D and 3D and a peculiar absence of halide redistribution in the dark that is only induced at higher temperature for the quasi-2D phase.

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Light-Induced Halide Segregation in 2D and Quasi-2D Mixed-Halide Perovskites

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Bibliografische nota

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